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Method for preparing formic acid and acetic acid by electrocatalytic reduction of carbon dioxide in heteropolyacid anion-acetonitrile-water ternary electrolyte system

A heteropolyacid anion, carbon dioxide technology, applied in electrolysis components, electrolysis process, electrolysis organic production and other directions, can solve problems such as large energy consumption, achieve mild reaction conditions, good electrochemical redox activity of polyoxometalates, simple steps

Active Publication Date: 2019-08-23
HARBIN INST OF TECH
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Problems solved by technology

[0005] The purpose of the present invention is to solve the problem of large energy consumption in the existing carbon dioxide reduction method, and provide a method for preparing formic acid and acetic acid by electrocatalytically reducing carbon dioxide in the heteropolyacid anion-acetonitrile-water ternary electrolyte system

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  • Method for preparing formic acid and acetic acid by electrocatalytic reduction of carbon dioxide in heteropolyacid anion-acetonitrile-water ternary electrolyte system
  • Method for preparing formic acid and acetic acid by electrocatalytic reduction of carbon dioxide in heteropolyacid anion-acetonitrile-water ternary electrolyte system
  • Method for preparing formic acid and acetic acid by electrocatalytic reduction of carbon dioxide in heteropolyacid anion-acetonitrile-water ternary electrolyte system

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specific Embodiment approach 1

[0026] Specific embodiment one: this embodiment is the method for preparing formic acid and acetic acid by electrocatalytic reduction of carbon dioxide in the heteropolyacid anion-acetonitrile-water ternary electrolyte system, specifically as follows:

[0027] 1. Preparation of ternary electrolyte solution: add acetonitrile into buffered aqueous solution, mix well to obtain acetonitrile-buffered aqueous solution, then add heteropolyacid anion room temperature ionic liquid to acetonitrile-buffered aqueous solution, and obtain heteropolyacid anion-acetonitrile after mixing -water ternary electrolyte solution; the pH of the buffered aqueous solution is 3.3 to 4.3; the volume ratio of the acetonitrile to the buffered aqueous solution is 3:2; the heteropolyacid in the heteropolyacid anion-acetonitrile-water ternary electrolyte solution The concentration of anions is 1.517mmol / L~2.275mmol / L;

[0028] 2. Preparation of acetonitrile-buffered aqueous solution: add acetonitrile into the...

specific Embodiment approach 2

[0034] Specific embodiment two: the difference between this embodiment and specific embodiment one is: the room temperature ionic liquid of heteropolyacid anion described in step one is made up of tetra-n-octylammonium bromide cation and heteropolyacid anion, and heteropolyacid anion The mol ratio of tetra-n-octyl ammonium bromide cation and heteropolyacid anion in the room temperature ionic liquid of polyacid anion is 7:1, and described tetra-n-octyl ammonium bromide cation chemical formula is [C 32 h 68 N] + , the chemical formula of the heteropolyacid anion is [SiW 9 V 3 o 40 ] 7- ;

[0035] Or the room temperature ionic liquid of heteropolyacid anion is made up of 1-dodecyl-3-methylimidazolium cation and heteropolyacid anion, and in the room temperature ionic liquid of heteropolyacid anion, 1-dodecyl-3-formazolium The mol ratio of imidazolium cation and heteropolyacid anion is 4:1, and described 1-dodecyl-3-methylimidazolium cation chemical formula is [C 16 h 31 N ...

specific Embodiment approach 3

[0040] Specific embodiment three: the difference between this embodiment and specific embodiment one or two is: when the room temperature ionic liquid of the heteropolyacid anion described in step one is composed of tetra-n-octylammonium bromide cation and heteropolyacid anion When composed, it is specifically prepared according to the following steps:

[0041] 1. Preparation of polyoxometalates:

[0042] ①, the Na 2 SiO 3 9H 2 O was dissolved in deionized water and Na was added with stirring 2 WO 4 2H 2 O, then add HCl solution with a concentration of 6mol / L, continue to stir and react for 10min, filter with glass sand, let the filtrate stand at 4°C for 2d~3d, precipitate white crystals, filter with glass sand, and dry at room temperature for 1d~ 2d, an intermediate product is obtained; the Na 2 SiO 3 9H 2 The mass of O and the volume ratio of deionized water are 60g:500mL; 2 SiO 3 9H 2 O and Na 2 WO 4 2H 2 The mass ratio of O is 60:362; The volume ratio of the...

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Abstract

The invention discloses a method for preparing formic acid and acetic acid by electrocatalytically reducing carbon dioxide in a heteropolyacid anion-acetonitrile-water ternary electrolyte system, and relates to a method for preparing formic acid and acetic acid by electrocatalytically reducing carbon dioxide. The purpose of the invention is to solve the problem of large energy consumption in the existing carbon dioxide reduction method. Method: 1. Preparation of ternary electrolyte solution; 2. Preparation of acetonitrile-buffered aqueous solution; 3. Electrocatalytic reduction: ①. Assembly; ②. Pre-electrolysis; ③. Electrolysis to obtain catholyte after electrolysis; 4. Separation to obtain formic acid and acetic acid. Advantages: the faradaic efficiency of the prepared formic acid is 20% to 90%, and the faradaic efficiency of the acetic acid is 5% to 70%. The invention is mainly used for the electrocatalytic reduction of carbon dioxide to prepare formic acid and acetic acid.

Description

technical field [0001] The invention relates to a method for preparing formic acid and acetic acid by electrocatalytically reducing carbon dioxide. Background technique [0002] carbon dioxide (CO 2 ) as a nontoxic and abundant carbon resource that can be converted into various valuable chemicals and fuels has attracted worldwide attention. However, carbon dioxide, as the highest valence form of carbon, has very high chemical thermodynamic and dynamic stability. At present, the solution to this problem mainly depends on the reduction of carbon dioxide under the conditions of high temperature, high pressure and catalyst addition, mainly including radiation reduction, chemical reduction, photocatalytic reduction, electrocatalytic reduction, and CO 2 Catalytic hydrogenation, etc. Among them, the advantage of the electrocatalytic reduction method is that the reaction can be realized at normal temperature and pressure, the reaction conditions are mild, the operation is simple, ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C25B3/04C25B3/25
CPCC25B3/25
Inventor 李春香查冰杰
Owner HARBIN INST OF TECH
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